Process for the manufacture of hydrogen and carbon-black.



R. Hx BROWNLEE & R. H. UHLINGER.

PROCESS FOR THE MANUFACTURE OF HYDROGEN AND CARBON BLACK. APPLICATION FILED JAN. 2|. 1914.

l ,276 4'7 a Patented Aug. 20, 1918 ROY H. BROWNLEE AND RoY H. UHLINGER, on PITTSBURGH, rENNsYLvANIA, AssIGN: oRs TO AMERICAN NrrRo-rRonuors COMPANY, or PITTSBURGH, PENNSYLVANIA,

A CORPORATION OF DELAWARE.

PROCESS FOR THE MANUFACTURE OF HYDROGEN AND CARBON -BLAGK.

Application filed January 21,1914. Serial No. 813,457.

. and without the use of complicated or expensive equipment.

The process most commonly employed for the manufacture of carbon black from natural gas is to eifect incomplete combustion of the gas in contact with a collecting exposed surface or surfaces, as a large iron plate or the like. Such a method is very wasteful, producing approximately one pound of carbon black from the possible average amount of thirty-five pounds of carbon theoretically I obtainable from one thousand ral gas.

This possible value, which is approximate, varies with the composition of the as.

In order to increase the yield 0 carbon and at the same time to produce and collect the resulting hydrogen, attempts have been made and patents have been issued for processes involving the decomposition of the gas by passing it through a highly heated tubular apparatus. Owing, however, to the impossibility of securing a material from which to make the tubes having the moss sary attributes of a highly refractory material capable of withstanding the unavoidable strains of expansion and contraction Without very heavy walls, good heat conductivity, and at the same time eficient. resistfeet of natuance to the decomposing action of carbon and hydrogen at very high temperatures,

none of these processes are commercially availabie, effioient or economical.

Other methods or processes for the making of hydrogen which have been used or tried have utilized the decomposing action of acids, upon metals, or the electrolysis of acids or alkalis; the action of strong alkalis upon certain metals, such as aluminum and zinc; the action of steam upon highly heat,

. ed metals, as iron; the passing of Water gas Specification of Letters Patent.

- tus adapted to the process.

Patented Aug. 20, rare.

over heated calcium carbid; the passing of Water gas and steam over heated lime; the passing of water gas over heated iron; and the liquefaction and rectification of water gas.

While several of these processes are or have been in successful operation, they are, except under specially favorable conditions, complicated and expensive operations, and

much more so than our process, while comparatively ineflicient as to results.

Generally stated, our process consists in highly heating a mass of highly refractory'material within a suitable Well insulated containing chamber and then passing through such chamber and hot refractory material a suitable hydrocarbon in the absence of air or other gases, or catalysts,or metals or metallic oxids. By this means the hydrocarbon is decomposed by coming into intimate contact with the highly heated refractory material, and is thereby decomposed,forming hydrogen and carbon.

The drawing shows in section an appara- The processis carried out as follows:

A vertical gas-tight furnace or chamber 2 is constructed, preferably with highly refractive linings 3 of suitable fire brick, and near the bottom is a supporting checker work 4 of similar material. A filling of irregular pieces of refractorymaterial 5 is contained within the body of the furnace, above the supporting checker work 4, or the entire inner part of the furnace may be built up of checker work of suitable refractory brick.

At the top of the furnace is a stack 6 provided with a suitable damper valve 7 for closing the stack and furnace gas-tight. In-

let pipes 8 for supplying the hydrocarbon,- as natural gas, are introduced through the upper portion of the furnace. The preswill be normally one pound. 0r more above atmospheric pressure, but owing to the more rapid reaction when a larger mass of gas is present, the pressure in thefurnace may be held at two or three atmospheres or higher.

A damper-controlled air conduit 10 having a damper or valve 11, and a gas pipe 12 having a controlling valve 13 are introduced sure of gas introduced through these pipes to chamber 9 below the checker work or readmitted from connections 12 and 10 for additional combustion and heating of the refractory contents of the furnace, preparatory to a repetition of the operation just described.

In case a liquid or volatilizable solid is used as a fuel at the base of the furnace, it may be sprayed or blown into the. combustion chamber 9.With an air blast. When the same kind of hydrocarbon is used at the top of the furnace, instead of gas, for the makingof hydrogen and lamp black, it may also be sprayed in under pressure, or atomized by the aid of compressed hydrogen, without air, so that only minute particles of the hydlrocarbon' will strike the hot checkerwor r.

Otherwise the entire checker work would soon be clogged with carbon, whereas, when either a gas or very fine spray is used, the finely divided carbon is carried down with the gas.

It will be readily understood that some carbon will necessarily adhere to the refractory material and the inner walls of the furnace, but by observing the above precau tions this will be reduced to a minimum. Such adhering carbon will be consumed in the next heating operation of the furnace. Owing to incidental traces of moisture in the hydrocarbon used and possible impurities such as metallic oxids in the refractory checker-work, which are however easily re ducible, some carbon monoxid is ordinarily produced during the operation of the furnace.

Where the expression absence of"catalysts, or absence ofmetals or metallic oxide, is used, it is understood to mean the absence of any supplemental or additional amounts of such, and that any such impurities as remain in the hydrogen are only such small amounts as the hydrocarbon may have have added to it, or from the walls of the furnace,v or from the refractory material contained in it. 7 7

Where the expression catalyst is used, it may be understood to refer to the excluded metals mentioned.

Where suitable natural gas is obtainable, such as Pennsylvania or West Virginia gas, this process is especially suited for making hydrogen, as each 1,000 feet of natural gas will produce on decomposition over 2,100 feet (cubic) of hydrogen.

When one cubic foot of Pennsylvania or West Virginia natural gas burns in air, somewhat over 1,100 B. T.'U. (British thermal units) of heat are produced, while only 145 B. 'l. U. are required to break up the hydrocarbons in a cubic foot of the same gas to form hydrogen and carbon black. This value, 145 B. T. U. also includes the heat necessary to raise the temperature of the gas to the temperature at which it will be decomposed by heat, in addition to the heat of decomposition of the gas.

That is to say that when one cubic foot of the gas burns, over 7.5 times as much heat is produced as is absorbed when one cubic foot of the same gas is decomposed by heat to form hydrogen and carbon black.

In case as large yieldsof carbon as possible are desired and the hydrogen is not re-' quired, for other purposes, the operation of heating'thefurnace may be effected by replacing the usual gas by hydrogen made in a prev1ous run of the furnace for that pur pose, and thus no natural gas will be used except for the actual decomposition of the same to form hydrogen and carbon black.

The importance of this procedure will be evident when it is pointed out that the heat of combustion of the hydrogen obtained from 1,000 cubic feet of Pennsylvania or \Vest Virginia natural gas is nearly four and a half times as much as the heat of decomposition of 1,000 cubic feet of the same natural gas.

By thorough insulation of the furnace, and

by using regenerators to save the heat thatis otherwise wasted in a simple furnace, such as is shown diagrammatically herewith, we may approach more nearly to the theoretical efiiciency.

But in practice, owing to the high tem peratures of 1,100 C. and over that must be maintained, the heat losses are necessarily .very considerable.

It is, of course, desirable to employ a refractory material for the inner lining and filling of the furnace, as withchecker work, using a substance that has the highest heat conductivity, and at the same time a high specific heat.

We claim: a

1. The process-of making carbon black and hydrogen consisting in decomposing a suitable hydrocarbon by bringing it into contact with highly heated refractory material within an inclosing chamber in the absence of air or catalyst, then cooling the decomposed elements to separate the carbon from the hydrogen, then removing and collecting the separated carbon, and then subjecting the hydrogen to cleansing operations to eliminate impurities.

2. lhe process of making carbon black and hydrogen consisting in heating refractory material within an inclosing chamber by combustion of a suitable fuel therein, then passing a suitable hydrocarbon through the chamber and in contact with the highly heated refractory material in the absence of air or catalyst, then passing the decomposed the sepereiecl carbon from x1e Gimme-I012 o" the hyclregen.

3. The prccess 0f makimg carben Week and hydrogen consisting in heatiq fiery material Within an incl sing cham der by combustien of a suitable iuel liirrezeiz'l then passing a, suitable hydrecerbsgl :bhmugh the and centect Wim. me hi; heated refl'actory materlai 1n the absence 1/).

from the hydrogen efiecting iechgniczl remove of the 03.1%011 and. then sunjecklg the hydrogela '50 Sun LLe elimina'ien 0f immu'.

4. The jorscess and h drc gen cansis'izing in he? ibofy material Wimin by wnfousti-ol? e swwssidg the wardly an ing and 301 ectmg th carbon suit the gaseous clrcvletwn 0:? the hydrogea an; a n subgectl ,ibhe ilg arogezl he am 12.31%

elimimulon of impuritiee "we nereun'te M we piesence m Lwe Wm 

